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Solid state core-exciton dynamics in NaCl observed by tabletop attosecond four-wave mixing spectroscopy

Journal Article · · Physical Review B
 [1];  [2];  [1];  [3];  [1];  [1];  [1]
  1. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Princeton Univ., NJ (United States)
  3. Univ. of California, Berkeley, CA (United States)
+ Show Author Affiliations
Nonlinear wave mixing in solids with ultrafast x-rays can provide insight into complex electronic dynamics of materials. Here, tabletop-based attosecond noncollinear four-wave mixing (FWM) spectroscopy using one extreme ultraviolet (XUV) pulse from high harmonic generation and two separately timed few-cycle near-infrared (NIR) pulses characterizes the dynamics of the Na+ L2,3 edge core-excitons in NaCl around 33.5 eV. An inhomogeneous distribution of core-excitons underlying the well-known doublet absorption of the Na+ Γ point core-exciton spectrum is deconvoluted by the resonance-enhanced nonlinear wave mixing spectroscopy. In addition, other dark excitonic states that are coupled to the XUV-allowed levels by the NIR pulses are characterized spectrally and temporally. Approximately <10fs coherence lifetimes of the core-exciton states are observed. Furthermore, the core-excitonic properties are discussed in the context of strong electron-hole exchange interactions, electron-electron correlation, and electron-phonon broadening. This investigation successfully indicates that tabletop attosecond FWM spectroscopies represent a viable technique for time-resolved solid state measurements.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
US Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES); William Keck Foundation
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1821669
Alternate ID(s):
OSTI ID: 1845298
Journal Information:
Physical Review B, Journal Name: Physical Review B Journal Issue: 24 Vol. 103; ISSN 2469-9950
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Electronic structure of atoms &amp; molecules
attosecond laser spectroscopy
electronic structure of atoms &amp; molecules
excitons
four-wave mixing
high-harmonic generation
insulators
ionic solids